The fine art collection was largely assembled by connoisseur Stephen C. Clark one of the Museum's greatest patrons. The collection contains some of the best examples of American landscape, history, and genre painting.

The works of Hudson River School painters are well represented and include Thomas Cole's Last of the Mohicans and Asher B. Durand's Hudson River Looking Toward the Catskills. Historical portraits include Gilbert Stuart's Joseph Brant, Ralph Earl's Baron Von Steuben, and Benjamin West's Robert Fulton, which all depict figures from New York's colorful history.

The Museum also owns a unique collection of life masks cast from the actual faces of famous Americans by John Henry Isaac Browere. Thomas Jefferson, John and John Quincy Adams, DeWitt Clinton, and Dolley Madison are among those in the collection.